International Journal of Greenhouse Gas Control 91 (2019) 102821

Contents lists available at ScienceDirect

International Journal of Greenhouse Gas Control

journal homepage: www.elsevier.com/locate/ijggc

Comparative environmental life cycle assessment of carbon capture for T

petroleum refining, ammonia production, and thermoelectric power
generation in the United States
Ben Younga, Michelle Krynockb, Derrick Carlsonb, Troy R. Hawkinsc, Joe Marriottb, Ben Morellia,
Matthew Jamiesonb, Gregory Cooneyb, Timothy J. Skoned,
⁎

a
Eastern Research Group, 110 Hartwell Avenue, Lexington, MA 02421, United States
b
Contractor to National Energy Technology Laboratory, 626 Cochrans Mill Road, P.O. Box 10940, Pittsburgh, PA 15236, United States
c
Systems Assessment Center, Energy Systems Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, IL 60439, United States
d
National Energy Technology Laboratory, 626 Cochrans Mill Road, P.O. Box 10940, Pittsburgh, PA 15236, United States

ARTICLE INFO ABSTRACT

Keywords: Understanding opportunities for carbon capture and storage (CCS) across sectors is important for choosing
Carbon capture among greenhouse gas mitigation strategies. This study explores the cradle-to-gate life cycle environmental
Petroleum refining impacts of amine solvent based carbon capture systems on U.S. ammonia production, petroleum refineries,
Ammonia supercritical and subcritical pulverized coal power plants, and natural gas combined cycle plants. We use
Thermoelectric power
publicly available data to create comprehensive life cycle inventories for petroleum refining and ammonia
Life cycle assessment
production for 2014. We use these processes and additional modeled carbon capture processes to compare
carbon capture on ammonia production and petroleum refining to inventories for coal and natural gas fired
electricity with carbon capture. This analysis found that particulate matter formation potential, eutrophication
potential, and water consumption increase in all sectors as a result of installation and operation of CCS tech-
nologies per kg CO2e abated, while the effect on acidification potential and particulate mater formation potential
is mixed. The differences in tradeoffs among systems are driven primarily by three factors: the combustion
emissions from fuel used to operate the capture unit, the upstream supply chain to obtain that fuel, and the
relative impact of the carbon capture unit on baseline flue gas emissions (i.e. possible co-benefits from capture).

1. Introduction
It has been argued that capturing carbon dioxide (CO2) from ex-
isting industrial systems offers a technologically feasible and relatively
non-disruptive option for reducing greenhouse gas (GHG) emissions
when compared with other proposed technologies in the near future
(Pollak et al., 2011; The National Coal Council, 2011; Wennersten et al.,
2015). Existing infrastructure and business organizational structures
embody significant investments which will likely persist long into the
future. Adapting these systems to capture and subsequently store CO2
emissions provides an opportunity to balance environmental and eco-
nomic performance.
However, implementing carbon capture and storage (CCS) will re-
sult in changes in environmental impacts along with reductions in GHG
emissions. Additional fuel or electricity consumption will be required to
operate the carbon capture unit and store the condensed CO2. The
upstream supply chains for the fuel and materials consumed by the
capture systems and during carbon storage will carry additional en-
vironmental impacts. As a result, life cycle thinking is necessary to track
the full range of possible impacts associated with the implementation of
CCS.
Understanding the opportunities and impacts associated with CCS
across sectors is important for choosing among GHG mitigation stra-
tegies. Performing a life cycle assessment (LCA) of mitigation strategies
enables a comparison of environmental tradeoffs that result from re-
duced CO2 emissions. Much of the current research in CCS in the United
States has focused on the impacts of capture from large sources of CO2
emissions such as power plants (Figueroa et al., 2008; Supekar and
Skerlos, 2017; Wang et al., 2017). Research into carbon capture from
smaller point sources of CO2, such as those from the industrial sector, is
more limited (Mora et al., 2017).
In this study, the environmental life cycle impacts of CCS are

⁎
Corresponding author.
E-mail address: timothy.skone@netl.doe.gov (T.J. Skone).

https://doi.org/10.1016/j.ijggc.2019.102821
Received 10 October 2018; Received in revised form 2 April 2019; Accepted 26 August 2019
Available online 23 October 2019
1750-5836/ © 2019 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/BY/4.0/).
B. Young, et al. International Journal of Greenhouse Gas Control 91 (2019) 102821

assessed across five U.S. systems. To do so, we use publicly available described in greater depth below, was modeled while maintaining the
data to develop comprehensive life cycle inventories for U.S. petroleum original reference flow. Additional detailed information on the supply
refining and ammonia production for the year 2014. Versions of these chains and life cycle stages for each system are provided in Tables SI-2
inventories that include a carbon capture unit were also developed to and SI-3 respectively.
enable comparisons of CCS in these industries to existing inventories for Life cycle impacts were assessed using the Tool for Reduction and
U.S. coal and natural gas fired electricity generation (NETL, 2018a, Assessment of Chemicals and other environmental Impacts (TRACI)
2018b, 2018c). Amine based solvents, such as monoethanolamine version 2.1 (U.S. EPA, 2014). A subset of impact categories are reported
(MEA), are the most common and well-researched method for post- herein: global warming potential (GWP), particulate matter formation
combustion carbon capture in the U.S. (Motazedi et al., 2017; Raynal potential (PMFP), photochemical smog formation potential (PSFP),
et al., 2011; Wang et al., 2017), so they are the focus of this study. eutrophication potential (EP), and acidification potential (AP). Water
Alternative methods of carbon capture, such as oxyfiring and alternate consumption (WC) is also reported as a summation of the inventory.
solvents, have been explored elsewhere (de Mello et al., 2013; The toxicity impact categories were not included because of re-
Johansson et al., 2012; Kuramochi et al., 2012). presentativeness concerns regarding the applicability of the USEtox
model underlying these impact categories within the TRACI model at
1.1. Systems of study this time. Where applicable, life cycle impacts are normalized across
impact categories; normalized impacts show the change in an impact
This study compares the potential environmental life cycle impacts category relative to total U.S. national impacts in 2008 (Ryberg et al.,
of post-combustion CCS across three U.S. industrial sectors: ammonia 2014).
production, petroleum refining, and electricity generation from natural A functional unit of 1 kg of CO2 equivalent (CO2e) abated, based on
gas combined cycle (NGCC), subcritical pulverized coal (SubPC), and Intergovernmental Panel on Climate Change (IPCC) Assessment Report
supercritical pulverized coal (SCPC) power plants. These systems were 5 using a 100-year time frame (Myhre et al., 2013), was used to com-
selected because they account for a significant share of U.S. point pare the impacts of CCS across the five production systems. This func-
source GHG emissions, present concentrated CO2 streams suitable for tional unit reflects the impacts of reducing life cycle GHG emissions by
carbon capture, represent a range of CO2 stream sizes, and are sup- 1 kg CO2e while maintaining the original reference flow of the product
ported by publicly available datasets. Table 1 compares these systems system, e.g. 1 kg ammonia or 1 MW h. Note that this refers to the net
on the basis of total U.S. sector CO2 emissions, the number of U.S. fa- reduction in CO2e; it considers the additional amount of CO2 which
cilities, and production volume with further information provide in must be captured to offset the additional CO2e associated with opera-
Table SI-1. In total, these systems account for 1.46 petagrams of CO2, or tion of the CCS process and its supply chains. Thus the functional units
26% of total CO2 emissions in the United States in 2014. On a per fa- of CO2 captured or stored and CO2e abated cannot be used inter-
cility basis, SCPC plants have the highest CO2 emissions per facility, changeably. This functional unit addresses the question “what is the
while NGCC plants have the lowest. This metric is relevant in the relative environmental impact associated with capturing carbon in one
context of deploying CCS in such a way that results in the most sig- sector versus another?”
nificant reductions in CO2 emissions per capture system installed. Total CO2e abated was calculated as the difference in life cycle GHG
emissions between the baseline scenario and CCS scenario (Equation 1).
1.2. System boundaries and scope Using this calculation, positive values reflect an increase in life cycle
impact X relative to a 1 kg reduction in CO2e over the life cycle of re-
Life cycle assessment (LCA) is a technique that quantifies the en- ference flow production. Negative values reflect a co-benefit associated
vironmental impacts associated with a process or product within a set of with CCS. A reduction in GHG emissions of 1 kg CO2e is explicitly re-
defined boundaries. This is achieved by calculating the material and quired by the approach taken in Equation 1 and the definition of the
energy requirements and emissions flows by life cycle stage – from functional unit, and therefore remains constant across the five systems
material extraction and processing through operations, use and dis- of study.
posal. Fig. 1 depicts the system boundaries used to conduct the LCA, Equation 1: Calculation of functional unit: 1 kg CO2e abated.
connecting life cycle inventory data discussed in detail in subsequent Ix , c Ix , n
sections. The life cycle stages and processes included for the production CO2 e abated
of the reference flow in the baseline scenario for each system include
extraction and processing of fuels, production of material inputs, and Where:
facility operations. In addition to this baseline scenario, a CCS scenario, Ix,c = Total life cycle impact X per unit of product with CCS
Ix,n = Total life cycle impact X per unit of product without CCS
Table 1 CO2e abated = GHG per unit of product without CCS − GHG per
Gate-to-gate CO2 emissions from systems of study, 2014. Emissions and facility unit of product with CCS
counts for each system were obtained from U.S. EPA’s Facility Level
Information on Greenhouse Gases Tool (FLIGHT) (U.S. EPA, 2016a) and U.S. 2. Inventory development - methodology
EPA’s Emissions & Generation Resource Integrated Database (eGRID) (U.S. EPA,
2017a). TWh: terawatt hour. 2.1. Baseline inventory for ammonia production and petroleum refining
System CO2 Emissions Facility Emissions per Sector Production
(Tg CO2) Count Facility (Tg) (Units) This study developed new, comprehensive inventory data for U.S.
i
ammonia production and petroleum refining based on national release
Ammonia 24 0.4% 23 1.1 11.4 Tg
Refinery 174 3% 142 1.2 5,780 million
inventories introduced in Table SI-4. New inventory data were also
barrelsii developed for several intermediate inputs to ammonia production,
SCPC 298 5% 41 7.3 302 TWh petroleum refining, and carbon capture unit processes including pet-
SubPC 800 14% 226 3.5 812 TWh roleum extraction and transport, zinc oxide production, ethylene oxide
NGCC 164 3% 185 0.90 406 TWh
production, and monoethanolamine production. Sources and methods
U.S. Totaliii 5,565 – – – –
for the development of new inventory data are summarized below with
i
Apodaca, 2016. additional details provided in the supporting information.
ii
1 U.S. barrel is approximately 159 L; U.S. EIA, 2016a. A data mining approach (Cashman et al., 2016) was used to gen-
iii
U.S. EPA (2017b). erate a national production-weighted average inventory for the

2
B. Young, et al.
Fig. 1. System boundaries for LCA of each system with and without CCS. Life cycle stages match those used for results display. Secondary fuel inputs for the electric
power sector are aggregated in the facility unit processes, but are separated out for the ammonia and petroleum refinery systems. The reference flow in each system is
maintained in both the baseline and CCS scenarios.
ammonia production and petroleum refining sectors. Reported facility
releases from various environmental datasets were standardized to re-
ported production. GHG emissions data were drawn from the Green-
house Gas Reporting Program (GHGRP) (U.S. EPA, 2016b). The Na-
tional Emissions Inventory (NEI) was used to estimate releases of
criteria and other air pollutants (U.S. EPA, 2016c). Releases to water
and transfers of toxic materials were sourced from Discharge Mon-
itoring Reports (DMR) and the Toxic Release Inventory (TRI) (U.S. EPA,
2016d, 2016e) (Table SI-4).
Quantities of manufactured ammonia and other fertilizer co-pro-
ducts were compiled for U.S. facilities from data collected by EPA’s
Chemical Data Reporting (CDR) program (U.S. EPA, 2012). Reported
2011 facility production from the CDR was scaled according to changes
in reported facility production capacity between 2011 and 2014, as
provided by the U.S. Geological Survey (Apodaca, 2016). Fuel con-
sumption at each facility was calculated from reported CO2 emissions
from the GHGRP and estimates of carbon intensity by fuel source (Table
SI-7). Other process inputs, such as electricity use, solvent consumption,
and natural gas feedstock were sourced from the literature due to lack
of facility-reported data (Althaus et al., 2007; U.S. EPA, 1993; Worrell
et al., 2000).
A significant share of ammonia manufactured at fertilizer facilities
is consumed on-site to generate other fertilizer products such as urea or
ammonium nitrate (Figs. SI-1). Following the guidance of ISO 14044
(ISO, 2006), emissions data provided within emissions inventories are
attributed to specific facility sub-processes where possible. Emissions of
greenhouse gases, criteria, and other hazardous air pollutants which
can be attributed to the ammonia production unit were allocated by
mass across gross ammonia production. Emissions attributed directly to
other products at the facility were excluded from the system. Un-
attributed, facility-wide emissions were allocated by mass across all
products (Table SI-5).
Annual crude petroleum refinery throughput was calculated using
refinery specific atmospheric crude distillation capacity (U.S. EIA,
2017a) adjusted by operating capacity utilization rate for each of the 12
3
International Journal of Greenhouse Gas Control 91 (2019) 102821
U.S. Petroleum Administration for Defense Districts (PADD) sub-regions
(U.S. EIA, 2017b). Refinery inputs and outputs were based on EIA re-
ports by PADD (U.S. EIA, 2016a, 2016b, 2016c). All input flows and
emissions were standardized to the total mass of petroleum product
output (Table SI-8).
Calculated national average release factors for each industrial sector
represent only those facilities that were successfully matched across the
relevant emissions and production datasets (Sengupta et al., 2015).
Total release of emissions from matched facilities were divided by total
facility production. For the petroleum refining sector, data from the
various emissions inventories cover between 78% and 99% of total
crude petroleum input to refineries. For the ammonia production
sector, emissions inventories from the matched facilities account for
between 61% and 87% of U.S. production capacity (Table SI-11).
2.2. Description of thermoelectric power systems
The thermoelectric power system inventory data used in this study
were drawn from ongoing research into power plant CCS by the
National Energy Technology Laboratory (NETL). NETL (2015) char-
acterized the financial and emissions impacts of CCS on the three power
plant configurations assessed in this study: SubPC, SCPC, and NGCC. As
modeled using Aspen Plus process modeling software, each plant gen-
erates a net power output of 550 MW at an 85% capacity factor. The
plants were configured to meet emissions limits for particulate matter
(PM), sulfur dioxide (SO2), and nitrogen oxides (NOx) based on reg-
ulatory standards outlined in the 2013 New Source Performance Stan-
dards (NETL, 2015). Mercury and hydrochloric acid emissions were
based on the 2013 Utility Mercury and Air Toxics Standards (NETL,
2015). The resulting inventory models were used as part of full life
cycle assessments, documented in three reports, one for each thermo-
electric power system (NETL, 2018b, 2018a, 2018c).
B. Young, et al. International Journal of Greenhouse Gas Control 91 (2019) 102821

2.3. Carbon capture and storage model

Amine-based Shell Cansolv Solvent system, MEA

CO2 is generated primarily from two sources in the ammonia pro-

used as a proxy for upstream production

duction process: combustion of fuel in the primary reformer and re-
moval of CO2 from the syngas stream (Strait and Nagvekar, 2010). The
CO2 emissions stream released from the syngas are already highly

Heat Recovery Steam Generator

purified, being approximately 99% CO2 (NETL, 2014). Syngas CO2

NGCC
emissions are regularly captured at ammonia facilities to produce urea
(NETL, 2014; Strait and Nagvekar, 2010); therefore they do not con-

0.074 KWh/kg CO2

0.23 MJ electricity
tribute to environmental emissions nor are they available for CCS. To

2.89 MJ/kg CO2

222 MT CO2/hr
2.66 MJ steam
best represent the marginal impacts of carbon capture in this model,
combustion emissions from the primary reformer were modeled as

emissions
being sent to an MEA carbon capture unit (Table SI-6). A techno-eco-

n.a.
nomic assessment of carbon capture on the syngas stream can be found
in NETL (2014).

Amine-based Shell Cansolv Solvent system, MEA

CO2 is emitted from numerous sources within a petroleum refinery
including various boilers, heaters, flares, the fluid catalytic cracker

used as a proxy for upstream production

(FCC), and the hydrogen production unit. There is an issue of scale and
diminishing returns for carbon capture, where including more sources
of emissions within the refinery in the capture system increases the
energy penalty for operating the system and decreases the concentra-

SubPC
tion of the CO2 in the emissions stream. This means that each additional
unit of CO2 captured costs more, in terms of both money and energy,

0.073 KWh/kg CO2

0.12 MJ electricity
than its predecessor. Fig. SI-2 shows FCC and hydrogen production unit

2.60 MJ/kg CO2

528 MT CO2/hr
2.48 MJ steam
emissions relative to combustion emissions and those of other proces-
sing units. An MEA carbon capture unit was modeled to process emis-

emissions
PC Boiler
sions from the FCC and hydrogen production units, due to their con-

n.a.
centrated share of CO2 emissions.
In the thermoelectric power systems, a Shell Cansolv amine-based

Compressed using an internally geared centrifugal compressor and transported for deep saline sequestration

Amine-based Shell Cansolv Solvent system, MEA

proprietary solvent system is modeled as capturing 90% of the CO2 in
the flue gas of the power plants. Energy used for the carbon capture

used as a proxy for upstream production

system is added to the auxillary load and reflected by the reduced
power efficiency at each plant (NETL, 2015).
Table 2 summarizes the characteristics of the carbon capture unit
for each system. The fuel mix used to satisfy the additional heat demand

* Energy use for the carbon capture unit does not include compression, which is tracked separately.
SCPC

in the ammonia production system was modeled assuming the esti-

mated national fuel mix for ammonia facilities (Table SI-7). The fuel
0.074 KWh/kg CO2
0.12 MJ electricity

mix for the petroleum refining capture unit was modeled to reflect EIA
2.60 MJ/kg CO2

550 MT CO2/hr
2.48 MJ steam

national reported fuel consumption data (Table SI-9).

Flue gas sent to the carbon capture unit must be low in SO2 to avoid
emissions
PC Boiler

contamination of the capture solvent (de Mello et al., 2009; Koornneef

n.a.

et al., 2010). Acceptable maximum SO2 flue gas concentrations for

amine-based capture units are between 1 and 10 ppm, which corre-
Fluid Catalytic Cracker and

sponds to reductions in flue stream SO2 of 75% to 98+% (de Mello

MEA-based system based

et al., 2009; Koornneef et al., 2010; NETL, 2015). In the petroleum

0.098 KWh/kg CO2

refining and ammonia production systems, a sodium hydroxide (NaOH)

Refinery

Facility fuel mix

28.6 MT CO2/hr
3.78 MJ/kg CO2
2.60 MJ/kg CO2

caustic solution was modeled to remove 95% of the SO2 emissions from
Hydrogen unit

on literature

the flue gas streams. In the power systems, an NaOH polishing scrubber
reduces SO2 to 1ppmv. In all cases, the caustic scrubber can also reduce
flue gas concentrations of nitrogen oxides by approximately 50%
(NETL, 2015). Due to the uncertainty regarding impacts on other flue
Comparison of carbon capture unit across systems.

Primary Reformer flue gas

emissions, no other direct reductions in flue gas emissions due to

MEA-based system based

carbon capture were considered for any of the capture systems. Minor
0.082 KWh/kg CO2

emissions of MEA degradation products, including ammonia and acet-

Ammonia

Facility fuel mix

20.5 MT CO2/hr
3.56 MJ/kg CO2
2.60 MJ/kg CO2

aldehyde, were modeled based on reported data from pilot projects

on literature

(Moser et al., 2011).

Energy use for carbon capture in the ammonia production and
stream

petroleum refinery systems reflects the best available public data for
systems of a comparable size and scope (de Mello et al., 2009; NETL,
Energy Use (Sensitivity)

2013). The Cansolv carbon capture systems modeled in the power

Size of Capture System
CO2 Capture Stream

Amine Solvent Type

plants represent a newer, more energy-efficient capture system than the

CO2 Specifications
CO2 Compression

capture system modeled in the ammonia production and petroleum

Energy Source
Energy Use*

refining facilities. To assess the sensitivity to improvements in energy

efficiency, a sensitivity analysis was performed on the capture unit
Table 2

energy use for ammonia production and petroleum refining. Although

we are unable to fully model an equivalent system due to data

4
B. Young, et al. International Journal of Greenhouse Gas Control 91 (2019) 102821

Fig. 2. Comparison of TRACI impacts due to CCS across sectors. Top: Relative change in impacts from baseline due to CCS per unit of reference flow. Sensitivity to
lower capture unit heat use in ammonia and petroleum systems is reflected by stars. Bottom: Changes in impacts due to CCS applied sector-wide. Impacts are
normalized to 2008 U.S. national totals (Ryberg et al., 2014).

restrictions on the proprietary capture system used in the power sys-
tems, we modeled a scenario in which the ammonia production and
petroleum refining capture systems use the same amount of energy per
kg CO2 captured as the PC power plants (2.6 MJ/kg CO2). This re-
presents a 27% and 31% reduction in energy use per kg CO2 captured
for the ammonia and petroleum facilities respectively.
Following capture, the CO2 is compressed to 2200 psia according to
specifications suitable for pipeline transport using an internally geared
centrifugal compressor (NETL, 2015). The CO2 is then transported via
pipeline to the aquifer and sequestered. All systems in this study op-
erate assuming identical pipeline and aquifer specifications.
3. Results
3.1. Carbon capture and storage across sectors
Fig. 2 shows the relative change in life cycle impact due to CCS in
each sector. The top panel of Fig. 2 shows the environmental changes

5
B. Young, et al.
Table 3
Impacts of CCS applied sector wide, in teragrams. Net GWP reduction reflects total GHGs abated relative to baseline GHG emissions. Abatement Efficiency measures
GHG emissions abated (CO2e) per unit of CO2 captured.
Baseline
Gate-to-gate Cradle-to-gate Gate-to-gate
CO2 Emitted GHGs (CO2e) CO2 Captured
Ammonia 11 16
Refinery 174 571
SCPC 247 273
SubPC 693 766
NGCC 154 189
Total 1,279 1,814
due to CCS in each sector and allows for an assessment of tradeoffs
across impact categories. For example, if one were interested in the
tradeoffs of CCS at the average U.S. ammonia facility, the top panel of
Fig. 2 shows that GWP decreases by approximately 25% with the ad-
dition of CCS at the expense of increased AP, PMFP, EP, PSFP, and WC.
The impacts of CCS per unit output are applied across the entire
sector for each of the five systems to assess the potential for sector-wide
impacts. This assessment makes no further assumptions about technical
or economic feasibility of CCS across each sector, but maintains total
sector output. The bottom panel of Fig. 2 shows the change in nor-
malized environmental impacts that result. For example, the addition of
CCS at all NGCC plants decreases total national GWP by 1.6% while
increasing PSFP by 0.2%. While the greatest potential for reductions in
GWP lie in the SubPC sector, CCS throughout this sector also would
result in the largest increases in impacts for PSFP, EP, and WC.
Across the five systems, approximately 1.2 petagrams of CO2 could
be sequestered, resulting in a net reduction of 880 Tg of CO2e (Table 3).
The coal power sectors reflect the highest possible life cycle GWP re-
duction at 70%. The coal power systems also have the highest possible
absolute potential GWP reductions sector-wide, at 190 and 533 Tg.
Across the five systems, the percent of direct facility CO2 emissions (i.e.
the limiting factor in a carbon capture scenario) relative to total GWP is
highest at the coal plants. Therefore, a greater percentage of life cycle
CO2 is available for capture. An alternative metric, abatement effi-
ciency, provides the life cycle GWP abatement per unit CO2 captured
instead of total GWP abatement or GWP abated per unit CO2e. This
metric shows the marginal benefits of capture for GWP are highest in
the NGCC system, as reflected by the highest abatement efficiency in
Table 3. This is because upstream GHG releases induced by capture at
an NGCC plant are lower than those for any other system, due to the use
of natural gas as the fuel source.
The historical justification for CCS relates to the climate benefits
that it can provide, but other types of impacts should also be con-
sidered. Fig. 3 highlights the tradeoffs that occur from the addition of
CCS to each system. The net change in impact under the CCS scenario is
standardized to the total CO2e abated over the life cycle of the CCS
scenario (Equation 1). Comparisons made across systems as in Fig. 3
should be viewed in the context of the overall magnitude of change
shown in Fig. 2. For example, the ammonia system shows a larger in-
crease in acidification per kg CO2e abated than the NGCC system
(Fig. 3, bottom right panel). However, the net impact on the system
overall is greater for the NGCC system; acidification increases 14% due
to CCS relative to the baseline compared to an increase of 6% for am-
monia (Fig. 2, top panel).
Fig. 3 makes clear that environmental impacts increase as a result of
implementing CCS, with the exception of PMFP and AP for the coal
electricity production systems. This is due to the additional energy re-
quired to operate the carbon capture system (Table 2). Energy use
generates impacts from both its upstream supply and combustion. As
described above, additional energy demand in the ammonia and pet-
roleum refinery systems is met with the same technologies and fuels
International Journal of Greenhouse Gas Control 91 (2019) 102821
CCS Applied Sector Wide Sector Results
Cradle-to-gate Net GWP Abatement
GHG Abated Reduction Efficiency
5.9 4.1 25% 69%
50 31 5% 62%
264 190 70% 72%
739 533 70% 72%
146 120 63% 82%
1,205 877
already used to provide heat in those industries. The ammonia system
relies almost exclusively on natural gas (Table SI-7), while the refinery
uses a mixture of refinery gas and natural gas, as well as purchased
electricity, purchased steam, and residual refinery products such as
distillate fuel oils (Table SI-9). The makeup of refinery fuels compared
to the natural gas burned in the ammonia facility (Table SI-12) or NGCC
results in higher environmental impacts, causing the on-site impacts to
be higher for EP, PSFP, and AP per kg CO2e abated (blue bars in Fig. 3).
The power plants also must increase generation to make up for the loss
in efficiency to operate the carbon capture system, causing increases in
impacts at the plant and upstream.
3.2. Global warming potential
In all sectors, the upstream GHG emissions due to acquisition and
processing of fuel for the carbon capture unit (upstream bar in Fig. 3)
reduce the abatement efficiency. Relative to the other sectors, the GWP
of the upstream supply chain for the additional fuel demand for carbon
capture at petroleum refineries is greatest. As a result, more CO2 must
be captured to achieve a net reduction of 1 kg CO2e. This reflects both
the specific supply chain for the fuels used at the refinery but also the
higher energy demand for the refinery carbon capture unit (Table 2).
The abatement efficiency reflects differences in energy demand at the
capture unit and the GHG releases upstream of the facility (Table 3).
Improving the energy efficiency of the carbon capture unit provides
dual benefits, by reducing the impacts from fuel acquisition and redu-
cing the need for offsetting carbon capture.
3.3. Particulate matter formation potential
PMFP in these systems is driven by release of SO2 and PM. Releases
of SO2 are common throughout the refinery life cycle and during coal
combustion. PM releases at the ammonia facility and refinery also
contribute. Carbon capture significantly reduces SO2 emissions at the
point of use. In the pulverized coal (PC) plants, increases in upstream
coal supply chain emissions, due to the increased input demands of
carbon capture, partially offset the benefits from SO2 reductions at the
facility. Similarly, SO2 emission reductions at ammonia facilities and
petroleum refineries are offset by increased PM releases from combus-
tion. The emissions from any additional combustion in the ammonia
and petroleum facilities do not pass through the carbon capture unit. As
a result, the decreases in SO2 emissions at the point of use are less
dramatic than those for the thermoelectric power systems, which do
capture the combustion emissions necessary to operate the capture
system. On net, PMFP increases at the facility when CCS is implemented
for the ammonia and petroleum systems, but decreases for the PC
power systems. Increased electricity consumption at ammonia facilities
and petroleum refineries also contributes significantly to higher PMFP
impacts. In the NGCC system, where PMFP is otherwise relatively in-
significant (NETL, 2018c), electricity use for saline aquifer sequestra-
tion drives two-thirds of the increase in PMFP. In the context of the
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B. Young, et al. International Journal of Greenhouse Gas Control 91 (2019) 102821

Fig. 3. Change in impact per kg CO2e abated over the life cycle. Total change in impacts for ammonia production and petroleum refining systems assuming lower
carbon capture unit heat use is reflected by stars. A net reduction in GWP of 1 kg CO2e is explicitly required by the approach used to calculate the function unit.

other industrial system life cycles, saline aquifer sequestration is not a
significant driver of PMFP; PM and SO2 releases during saline aquifer
sequestration contribute between 5% and 8% of the net increase in
PMFP for the ammonia and petroleum refinery systems. This is further
shown in Figs. SI-6 and SI-7.
the flue stream, but this effect is partially offset by increased NOx
emissions from combustion of fuels to operate the capture system.
Higher NOx emissions from combustion, a smaller life cycle impact
from reduced NOx scrubbing at the capture unit, and a heavy reliance
on natural gas fuel result in the highest life cycle impacts at the pet-
roleum refinery.

3.4. Photochemical smog formation potential

PSFP primarily results from release of NOx. Natural gas processing
results in significant releases of NOx, and therefore the systems that use
natural gas to provide heat for carbon capture demonstrate increases in
upstream impacts. The carbon capture unit reduces NOx emissions from
3.5. Eutrophication potential
Like PSFP, EP is driven strongly by emissions of NOx. Systems that
depend on natural gas to provide energy for the carbon capture unit
show increases in upstream NOx emissions and a corresponding

7
B. Young, et al.
increase in EP. Ammonia air emissions, a degradation product of MEA,
are responsible for 14% and 12% respectively of EP at the facility gate
with CCS for the ammonia and petroleum refinery systems; these MEA
ammonia degradation products more than offset reductions in NOx
emissions from the carbon capture unit. However, the net effects of this
release are minor in the context of the overall life cycle. The net change
in eutrophication at the facility gate would be slightly negative without
this degradation byproduct, but the net life cycle impact per kg CO2e
abated would remain positive. In the context of the entire ammonia
production life cycle, CCS increases EP by 3% per kg ammonia pro-
duced (Fig. 2, top panel).
3.6. Acidification potential
AP predominantly results from the release of NOx and SO2. At the
PC plants, net AP at the facility gate is negative due to CCS. As was
described in the context of PMFP from SO2, the additional NOx emis-
sions generated from combuston for carbon capture at the power plants
are more limited due to their passage through the capture system. Only
for the PC systems is the net benefit of CCS at the facility gate enough to
offset increased upstream supply chain impacts. Emissions of NOx
during natural gas extraction and processing contribute considerably to
AP under the CCS scenario for ammonia, petroleum refineries, and
NGCC power plants.
3.7. Water consumption
For each system with CCS, WC increases on-site due to the cooling
load incurred by the carbon capture unit. The ASPEN power plant
models include an integrated cooling system specific to each power
plant configuration. The ammonia production and petroleum refining
sectors use a single estimate of water use from literature assuming no
integration with the system because the plant configurations are not
specified (de Mello et al., 2009). All the systems see an increase in WC
upstream due to the additional material and energy demands of the
carbon capture unit. In the ammonia and refinery systems, this increase
is primarily due to the electricity demand of the carbon capture unit.
As a general trend, the environmental impacts of adding carbon
capture to power plants (both coal and natural gas) are lower than the
impacts of adding capture to smaller industrial sources of CO2. More
detail on the ammonia and petroleum industry life cycle results can be
found in the Supporting Information, where life cycle TRACI impacts
for the ammonia system, based on a functional unit of 1 kg of ammonia
product, and the petroleum system, based on a functional unit of 1 kg of
petroleum product, are broken down in more detail. Additional details
for the SubPC, SCPC and NGCC life cycle analyses with a functional unit
of 1 MW h can be found in their respective reports (NETL, 2018b,
2018a, 2018c).
4. Discussion
This study identified possible co-benefits from carbon capture at the
facility gate, in particular in reductions of SO2 and NOx from flue gas.
The relative impact of these co-benefits on the entire life cycle depends
on the magnitude of the reduction at the plant. In the case of the coal
power plants, the plant itself is the primary source of life cycle SO2
emissions. As a result, a greater percentage of life cycle emissions can
be passed through the capture unit, and removed, resulting in a net
decrease in AP and PMFP. The co-benefits are likely to be greatest
where baseline emissions are highest. In the ammonia production,
petroleum refining, and NGCC systems, reductions in SO2 at the capture
unit are more than offset by increases in the upstream fuel supply.
There is significant uncertainty around the potential for reduction in
additional emissions by the capture unit, such as particulate matter,
nitrous oxide, and volatile organic compounds. However, across all
systems, life cycle impacts are driven by emissions of NOx and SO2, and
8
International Journal of Greenhouse Gas Control 91 (2019) 102821
so the capture of additional flows is unlikely to impact the life cycle
results.
Direct impacts of the capture unit, through the solvent supply chain
and solvent emissions, and carbon sequestration stage are dwarfed by
impacts from the upstream energy supply chain and combustion. Better
data on the possible degradation products of the MEA solvent are
needed, but are unlikely to significantly alter the life cycle impact re-
sults.
While the system boundaries, background data, and modeling de-
cisions are the same between systems, they ultimately reflect different
things: the petroleum refinery and ammonia systems represent a top
down national inventory while the power plants represent a specific
power plant run through a detailed thermodynamic model. As a result,
we have chosen not to represent combined uncertainty or variability in
this analysis. This decision is further detailed in the SI, with a com-
pleted variability analysis of the ammonia and petroleum systems in-
cluded (Fig. SI-8).
It is clear from this analysis that accounting for the upstream fuel
supply chains required by CCS is necessary to assess the environmental
tradeoffs. Furthermore, this analysis identified that the magnitude of
these tradeoffs vary across sectors. PSFP, EP, and WC increase in all
sectors as a result of installation and operation of CCS technology. The
net effect on environmental impact is mixed for AP and PMFP (Fig. 2).
The differences in tradeoffs among systems are driven primarily by
three factors: the combustion emissions from fuel used to operate the
capture unit, the upstream supply chain to obtain that fuel, and the
relative impact of the carbon capture unit on baseline flue gas emissions
(i.e. possible co-benefits from capture).
The results of the sensitivity analysis reinforce the importance of
using energy efficient carbon capture systems. The total life cycle im-
pacts are reduced significantly in all impact categories – typically
20–30% but as high as a 60% reduction in PSFP for ammonia produc-
tion – when the energy efficiency is improved for the ammonia and
petroleum systems. In the case of PSFP, this change even re-orders
which systems have the smallest tradeoffs; the ammonia system, which
normally has the largest PSFP impact per kg CO2e abated, has the
smallest increase in PSFP when the sensitivity to energy efficiency is
performed. Investigating the viability of a Shell Cansolv capture system
in a petroleum refinery or ammonia facility was outside the scope of
this study, but using a carbon capture system which uses the same
energy efficiency does greatly improve the environmental life cycle of
the system. Improved efficiency reduces the magnitude of emissions at
the facility while also limiting impacts upstream. However, these sen-
sitivity results do not negate our conclusion that, overall, the PC power
plants have the lowest environmental tradeoffs associated with adding
amine-based CCS systems.
4.1. Conclusions and future work
While our findings support that amine-based post-combustion CCS
results in lower overall environmental impacts across multiple impact
categories for thermoelectric power plants compared to ammonia and
refinery industrial operations, CCS commercial viability is a complex
decision based on technical, economic, and environmental viability.
This study only addresses life cycle environmental performance of
amine-based post-combustion technology differences when applied to
thermoelectric power plants and ammonia and refinery industrial op-
erations. Future research should focus on alternative and emerging
carbon capture technologies and additional industrial sources of CO2
such as cement and steel production. More work should be done on the
power plant systems to ensure the data coverage is more similar to the
ammonia and petroleum systems.
Disclaimer
This analysis was prepared by the Office of Fossil Energy (FE) for
B. Young, et al.
the United States Department of Energy (DOE), National Energy
Technology Laboratory (NETL). This work was completed under DOE
NETL Contract Number DE-FE0025912. This study was prepared as an
account of work sponsored by an agency of the United States
Government. Neither the United States Government nor any agency
thereof, nor any of their employees, makes any warranty, express or
implied, or assumes any legal liability or responsibility for the accuracy,
completeness, or usefulness of any information, apparatus, product, or
process disclosed, or represents that its use would not infringe privately
owned rights. Reference herein to any specific commercial product,
process, or service by trade name, trademark, manufacturer, or other-
wise does not necessarily constitute or imply its endorsement, re-
commendation, or favoring by the United States Government or any
agency thereof. The views and opinions of authors expressed herein do
not necessarily state or reflect those of the United States Government or
any agency thereof.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Appendix A. Supplementary data
Supplementary material related to this article can be found, in the
online version, at doi:https://doi.org/10.1016/j.ijggc.2019.102821.
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